This paper describes the microstructural evolution in an alloy of uranium with 10 wt.% molybdenum (U10Mo), with minor addition of a third alloying element, namely, Cr, Ni, or Co, at 0.2 wt.%. The microstructures of arc-melted buttons in the as-cast condition show significant Mo segregation. The segregation behavior of Cr, Ni, and Co was investigated through detailed scanning electron microscope imaging. A homogenization heat treatment at 900°C for 48 h results in uniform Mo distribution and associated grain growth in all of the four alloys that were fabricated. Further, formation of multiple phases was noted in U-9.8 wt.% Mo-0.2 wt.% Ni and U-9.8 wt.% Mo-0.2 wt.% Co alloys after the homogenization annealing step. The greatest grain-boundary-initiated eutectoid transformation as measured by % volume fraction was observed when the homogenized U-9.8 wt.% Mo-0.2 wt.% Ni alloy was aged at 500°C for 20 h. The least eutectoid transformation occurred in U10Mo.